Advanced Energy Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Июнь 25, 2024
Abstract
Metal‐organic
frameworks
(MOFs)
have
exhibited
encouraging
catalytic
activity
for
the
oxygen
evolution
reaction
(OER),
a
crucial
process
water
electrolysis
to
produce
green
hydrogen.
Nonetheless,
distinguishing
source
of
and
establishing
structure‐composition‐property
relationships
MOFs
during
OER
processes
remain
challenging.
Here,
first
time,
operando
X‐ray
absorption
spectroscopy
(XAS)
is
utilized
monitor
structural
identify
active
components
ferrocene‐based
(Ni‐Fc)
OER.
Ligand‐defect‐rich
Ni‐Fc
synthesized
via
co‐deposition
method.
After
electrochemical
activation,
exhibits
superior
electrocatalytic
(228
mV
at
10
mA
cm
−2
in
0.1
m
KOH),
which
highly
competitive
compared
with
state‐of‐the‐art
electrocatalysts.
Operando
XAS
analysis
ex‐situ
characterizations
reveal
reconstruction
into
amorphous
NiFe‐catalysts
(a‐NiFe)
activation
process,
further
real
phases
(a‐NiFe‐C)
under
potential
greater
than
1.45
V
(vs
RHE).
In
phases,
in‐situ
formed
deprotonated
oxygen‐defected
Ni
oxyhydroxide
analogues
act
as
sites,
while
Fe
hydroxide
derived
from
ligands
optimize
electronic
structure
sites
improving
activity.
Density
functional
theory
(DFT)
indicates
reduced
energy
barrier
a‐NiFe‐C
pristine
MOFs,
supporting
improved
latter.
Chemical Reviews,
Год журнала:
2024,
Номер
124(7), С. 3694 - 3812
Опубликована: Март 22, 2024
Electrocatalytic
water
splitting
driven
by
renewable
electricity
has
been
recognized
as
a
promising
approach
for
green
hydrogen
production.
Different
from
conventional
strategies
in
developing
electrocatalysts
the
two
half-reactions
of
(e.g.,
and
oxygen
evolution
reactions,
HER
OER)
separately,
there
growing
interest
designing
bifunctional
electrocatalysts,
which
are
able
to
catalyze
both
OER.
In
addition,
considering
high
overpotentials
required
OER
while
limited
value
produced
oxygen,
is
another
rapidly
exploring
alternative
oxidation
reactions
replace
hybrid
toward
energy-efficient
generation.
This
Review
begins
with
an
introduction
on
fundamental
aspects
splitting,
followed
thorough
discussion
various
physicochemical
characterization
techniques
that
frequently
employed
probing
active
sites,
emphasis
reconstruction
during
redox
electrolysis.
The
design,
synthesis,
performance
diverse
based
noble
metals,
nonprecious
metal-free
nanocarbons,
overall
acidic
alkaline
electrolytes,
thoroughly
summarized
compared.
Next,
their
application
also
presented,
wherein
anodic
include
sacrificing
agents
oxidation,
pollutants
oxidative
degradation,
organics
upgrading.
Finally,
concise
statement
current
challenges
future
opportunities
presented
hope
guiding
endeavors
quest
sustainable
Advanced Materials,
Год журнала:
2023,
Номер
35(30)
Опубликована: Апрель 18, 2023
Rare-earth
(RE)-based
transition
metal
oxides
(TMO)
are
emerging
as
a
frontier
toward
the
oxygen
evolution
reaction
(OER),
yet
knowledge
regarding
their
electrocatalytic
mechanism
and
active
sites
is
very
limited.
In
this
work,
atomically
dispersed
Ce
on
CoO
successfully
designed
synthesized
by
an
effective
plasma
(P)-assisted
strategy
model
(P-Ce
SAs@CoO)
to
investigate
origin
of
OER
performance
in
RE-TMO
systems.
The
P-Ce
SAs@CoO
exhibits
favorable
with
overpotential
only
261
mV
at
10
mA
cm-2
robust
electrochemical
stability,
superior
individual
CoO.
X-ray
absorption
spectroscopy
situ
Raman
reveal
that
Ce-induced
electron
redistribution
inhibits
CoO
bond
breakage
CoOCe
unit
site.
Theoretical
analysis
demonstrates
gradient
orbital
coupling
reinforces
covalency
Ce(4f)─O(2p)─Co(3d)
site
optimized
Co-3d-eg
occupancy,
which
can
balance
adsorption
strength
intermediates
turn
reach
apex
theoretical
maximum,
excellent
agreement
experimental
observations.
It
believed
establishment
Ce-CoO
set
basis
for
mechanistic
understanding
structural
design
high-performance
catalysts.
Energy & Environmental Science,
Год журнала:
2023,
Номер
16(4), С. 1384 - 1430
Опубликована: Янв. 1, 2023
This
review
presents
the
state-of-the-art
MEAs,
including
key
components
and
preparation
technologies.
Especially,
overall
design
strategies
of
MEAs
are
discussed
to
promote
high-performance
alkaline
water
electrolysis.
Nature Communications,
Год журнала:
2023,
Номер
14(1)
Опубликована: Сен. 20, 2023
Renewable
energy-based
electrocatalytic
oxidation
of
organic
nucleophiles
(e.g.methanol,
urea,
and
amine)
are
more
thermodynamically
favourable
and,
economically
attractive
to
replace
conventional
pure
water
electrooxidation
in
electrolyser
produce
hydrogen.
However,
it
is
challenging
due
the
competitive
oxygen
evolution
reaction
under
a
high
current
density
(e.g.,
>300
mA
cm-2),
which
reduces
anode
electrocatalyst's
activity
stability.
Herein,
taking
lower
energy
cost
urea
as
model
reaction,
we
developed
oxyanion-engineered
Nickel
catalysts
inhibit
competing
during
achieving
an
ultrahigh
323.4
cm-2
at
1.65
V
with
99.3
±
0.4%
selectivity
N-products.
In
situ
spectra
studies
reveal
that
such
generated
oxyanions
not
only
OH-
adsorption
guarantee
coverage
reactant
on
active
sites
avoid
but
also
accelerate
urea's
C
-
N
bond
cleavage
form
CNO
intermediates
for
facilitating
reaction.
Accordingly,
comprehensive
mechanism
behaviour
between
boost
dynamic
change
Ni
was
proposed.
This
work
presents
feasible
route
high-efficiency
even
various
reactions
practical
applications.
Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
62(17)
Опубликована: Март 2, 2023
The
construction
of
high-activity
and
low-cost
electrocatalysts
is
critical
for
efficient
hydrogen
production
by
water
electrolysis.
Herein,
we
developed
an
advanced
electrocatalyst
anchoring
well-dispersed
Ir
nanoparticles
on
nickel
metal-organic
framework
(MOF)
Ni-NDC
(NDC:
2,6-naphthalenedicarboxylic)
nanosheets.
Benefiting
from
the
strong
synergy
between
MOF
through
interfacial
Ni-O-Ir
bonds,
synthesized
Ir@Ni-NDC
showed
exceptional
electrocatalytic
performance
evolution
reaction
(HER),
oxygen
(OER)
overall
splitting
in
a
wide
pH
range,
superior
to
commercial
benchmarks
most
reported
electrocatalysts.
Theoretical
calculations
revealed
that
charge
redistribution
bridge
induced
optimization
H2
O,
OH*
H*
adsorption,
thus
leading
accelerated
electrochemical
kinetics
HER
OER.
This
work
provides
new
clue
exploit
bifunctional
pH-universal
splitting.
Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
62(40)
Опубликована: Авг. 15, 2023
Abstract
Heteroatom
doping
has
emerged
as
a
highly
effective
strategy
to
enhance
the
activity
of
metal‐based
electrocatalysts
toward
oxygen
evolution
reaction
(OER).
It
is
widely
accepted
that
does
not
switch
OER
mechanism
from
adsorbate
(AEM)
lattice‐oxygen‐mediated
(LOM),
and
enhanced
attributed
optimized
binding
energies
intermediates.
However,
this
seems
inconsistent
with
fact
overpotential
doped
(<300
mV)
considerably
smaller
than
limit
AEM
(>370
mV).
To
determine
origin
inconsistency,
we
select
phosphorus
(P)‐doped
nickel‐iron
mixed
oxides
model
observe
enhances
covalency
metal‐oxygen
bonds
drive
pathway
transition
LOM,
thereby
breaking
adsorption
linear
relation
between
*OH
*OOH
in
AEM.
Consequently,
obtained
P‐doped
display
small
237
mV
at
10
mA
cm
−2
.
Beyond
P,
similar
also
observed
on
sulfur
doping.
These
findings
offer
new
insights
into
substantially
originating
heteroatom
Energy & Fuels,
Год журнала:
2023,
Номер
37(4), С. 2608 - 2630
Опубликована: Фев. 2, 2023
Hydrogen
is
believed
to
be
one
of
the
essential
clean
secondary
energy
sources
in
structure
revolution
both
industry
and
daily
life.
Driven
by
renewable
electricity
such
as
solar
wind
power,
water
electrolysis
for
hydrogen
production
deemed
main
processes
green
future
academia
industry.
Transition
metal
chalcogenides
(TMCs)
are
promising
candidates
replace
noble
metals
earth-abundant
electrocatalysts
splitting.
However,
it
remains
challenging
further
improve
electrocatalytic
activity
long-term
stability
TMCs,
especially
a
practical
electrolyzer.
This
Review
summarizes
recent
advances
strategies
optimizing
activities
TMCs
toward
splitting
well
latest
investigations
on
surface
reconstructions
during
electrolysis.
The
performances
cells
particularly
discussed.
Finally,
concluding
remark
perspective
provided,
we
hope
inspire
works
this
area,
narrowing
gap
between
material
design
application.
